Application of discrete solvent reaction field model with self-consistent atomic charges and atomic polarizabilities to calculate the χ(1) and χ(2) of organic molecular crystals

• Published in: Chemical physics letters Vol. 691; pp. 8 - 13
• Main Author: Lu, Shih-I
• Format: Journal Article
• Language: English
• Published: Elsevier B.V 01.01.2018
• ISSN: 0009-2614; 1873-4448
• DOI: 10.1016/j.cplett.2017.10.036

[Display omitted] •Linear and nonlinear optical properties of organic molecular crystals from discrete reaction solvent filed model.•Impact of updating atomic polarizabilities on the linear and second-order nonlinear susceptibilities.•Size and shape effects of target cell on the linear and second-order nonlinear susceptibilities. We use the discrete solvent reaction field model to evaluate the linear and second-order nonlinear optical susceptibilities of 3-methyl-4-nitropyridine-1-oxyde crystal. In this approach, crystal environment is created by supercell architecture. A self-consistent procedure is used to obtain charges and polarizabilities for environmental atoms. Impact of atomic polarizabilities on the properties of interest is highlighted. This approach is shown to give the second-order nonlinear optical susceptibilities within error bar of experiment as well as the linear optical susceptibilities in the same order as experiment. Similar quality of calculations are also applied to both 4-N,N-dimethylamino-3-acetamidonitrobenzene and 2-methyl-4-nitroaniline crystals.